skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Picosecond energy transfer and multiexciton transfer outpaces Auger recombination in binary CdSe nanoplatelet solids

Abstract

Fluorescence resonance energy transfer (FRET) enables photosynthetic light harvesting1, wavelength down-conversion in light-emitting diodes (LEDs)2, and optical bio-sensing schemes3. The rate and efficiency of this donor to acceptor transfer of excitation between chromophores dictates the utility of FRET and can unlock new device operation motifs including quantum-funnel solar cells4, non-contact chromophore pumping from a proximal LED5, and drastically reduced gain thresholds6. However, the fastest reported FRET time constants involving spherical quantum dots (QDs) (0.12-1 ns7-9), do not outpace biexciton Auger recombination (0.01-0.1 ns)10, which impedes multiexciton-driven applications including electrically-pumped lasers11 and carrier-multiplication-enhanced photovoltaics.12,13 Few-monolayer thick semiconductor nano-platelets (NPLs) with tens-of-nanometer diameters14 exhibit intense optical transitions14 and hundreds-of-picosecond Auger recombination15,16, but heretofore lack FRET characterizations. We examine binary CdSe NPL solids and show that inter-plate FRET (~6-23 ps, presumably for co-facial arrangements) can occur 15-50 times faster than Auger recombination15,16 and demonstrate multiexcitonic FRET, making such materials ideal candidates for advanced technologies.

Authors:
; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Science Foundation (NSF); USDOE Office of Science - Office of Basic Energy Sciences - Scientific User Facilities Division
OSTI Identifier:
1392336
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 14; Journal Issue: 5; Journal ID: ISSN 1476-1122
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English

Citation Formats

Rowland, Clare E., Fedin, Igor, Zhang, Hui, Gray, Stephen K., Govorov, Alexander O., Talapin, Dmitri V., and Schaller, Richard D. Picosecond energy transfer and multiexciton transfer outpaces Auger recombination in binary CdSe nanoplatelet solids. United States: N. p., 2015. Web. doi:10.1038/NMAT4231.
Rowland, Clare E., Fedin, Igor, Zhang, Hui, Gray, Stephen K., Govorov, Alexander O., Talapin, Dmitri V., & Schaller, Richard D. Picosecond energy transfer and multiexciton transfer outpaces Auger recombination in binary CdSe nanoplatelet solids. United States. https://doi.org/10.1038/NMAT4231
Rowland, Clare E., Fedin, Igor, Zhang, Hui, Gray, Stephen K., Govorov, Alexander O., Talapin, Dmitri V., and Schaller, Richard D. Mon . "Picosecond energy transfer and multiexciton transfer outpaces Auger recombination in binary CdSe nanoplatelet solids". United States. https://doi.org/10.1038/NMAT4231.
@article{osti_1392336,
title = {Picosecond energy transfer and multiexciton transfer outpaces Auger recombination in binary CdSe nanoplatelet solids},
author = {Rowland, Clare E. and Fedin, Igor and Zhang, Hui and Gray, Stephen K. and Govorov, Alexander O. and Talapin, Dmitri V. and Schaller, Richard D.},
abstractNote = {Fluorescence resonance energy transfer (FRET) enables photosynthetic light harvesting1, wavelength down-conversion in light-emitting diodes (LEDs)2, and optical bio-sensing schemes3. The rate and efficiency of this donor to acceptor transfer of excitation between chromophores dictates the utility of FRET and can unlock new device operation motifs including quantum-funnel solar cells4, non-contact chromophore pumping from a proximal LED5, and drastically reduced gain thresholds6. However, the fastest reported FRET time constants involving spherical quantum dots (QDs) (0.12-1 ns7-9), do not outpace biexciton Auger recombination (0.01-0.1 ns)10, which impedes multiexciton-driven applications including electrically-pumped lasers11 and carrier-multiplication-enhanced photovoltaics.12,13 Few-monolayer thick semiconductor nano-platelets (NPLs) with tens-of-nanometer diameters14 exhibit intense optical transitions14 and hundreds-of-picosecond Auger recombination15,16, but heretofore lack FRET characterizations. We examine binary CdSe NPL solids and show that inter-plate FRET (~6-23 ps, presumably for co-facial arrangements) can occur 15-50 times faster than Auger recombination15,16 and demonstrate multiexcitonic FRET, making such materials ideal candidates for advanced technologies.},
doi = {10.1038/NMAT4231},
url = {https://www.osti.gov/biblio/1392336}, journal = {Nature Materials},
issn = {1476-1122},
number = 5,
volume = 14,
place = {United States},
year = {2015},
month = {3}
}

Works referenced in this record:

Picosecond Energy Transfer in Quantum Dot Langmuir−Blodgett Nanoassemblies
journal, December 2003


Förster Resonance Energy Transfer Investigations Using Quantum-Dot Fluorophores
journal, January 2006


Carrier Cooling in Colloidal Quantum Wells
journal, February 2012


Electronic Energy Transfer in CdSe Quantum Dot Solids
journal, February 1996


Optical Gain and Stimulated Emission in Nanocrystal Quantum Dots
journal, October 2000


Universal Size-Dependent Trend in Auger Recombination in Direct-Gap and Indirect-Gap Semiconductor Nanocrystals
journal, May 2009


Analysis of Shape and Dimensionality Effects on Fluorescence Resonance Energy Transfer from Nanocrystals to Multiple Acceptors
journal, February 2013


Solar Cells Using Quantum Funnels
journal, September 2011


Bimolecular Auger Recombination of Electron–Hole Pairs in Two-Dimensional CdSe and CdSe/CdZnS Core/Shell Nanoplatelets
journal, October 2013


Fast energy transfer in layer-by-layer assembled CdTe nanocrystal bilayers
journal, April 2004


Peak External Photocurrent Quantum Efficiency Exceeding 100% via MEG in a Quantum Dot Solar Cell
journal, December 2011


Two-Dimensional Growth of CdSe Nanocrystals, from Nanoplatelets to Nanosheets
journal, February 2013


Spectrally Resolved Dynamics of Energy Transfer in Quantum-Dot Assemblies: Towards Engineered Energy Flows in Artificial Materials
journal, October 2002


Multiple Exciton Generation in Colloidal Nanocrystals
journal, December 2013


Low-Threshold Stimulated Emission Using Colloidal Quantum Wells
journal, April 2014


Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems
journal, April 2007


Colloidal nanoplatelets with two-dimensional electronic structure
journal, October 2011


Improved performance and stability in quantum dot solar cells through band alignment engineering
journal, May 2014


Quasi 2D Colloidal CdSe Platelets with Thicknesses Controlled at the Atomic Level
journal, December 2008


Generalized Theory of Förster-Type Nonradiative Energy Transfer in Nanostructures with Mixed Dimensionality
journal, May 2013

  • Hernández-Martínez, Pedro Ludwig; Govorov, Alexander O.; Demir, Hilmi Volkan
  • The Journal of Physical Chemistry C, Vol. 117, Issue 19
  • https://doi.org/10.1021/jp402242y

Electronic Structure and Exciton–Phonon Interaction in Two-Dimensional Colloidal CdSe Nanosheets
journal, May 2012


Energy-transfer pumping of semiconductor nanocrystals using an epitaxial quantum well
journal, June 2004